Chemical Reviews,
Journal Year:
2022,
Volume and Issue:
123(9), P. 5948 - 6002
Published: Dec. 27, 2022
The
surface
and
interface
coordination
structures
of
heterogeneous
metal
catalysts
are
crucial
to
their
catalytic
performance.
However,
the
complicated
make
it
challenging
identify
molecular-level
structure
active
sites
thus
precisely
control
To
address
this
challenge,
atomically
dispersed
(ADMCs)
ligand-protected
precise
clusters
(APMCs)
have
been
emerging
as
two
important
classes
model
in
recent
years,
helping
build
bridge
between
homogeneous
catalysis.
This
review
illustrates
how
chemistry
these
types
determines
performance
from
multiple
dimensions.
section
ADMCs
starts
with
local
at
metal–support
interface,
then
focuses
on
effects
coordinating
atoms,
including
basicity
hardness/softness.
Studies
also
summarized
discuss
cooperativity
achieved
by
dual
remote
effects.
In
APMCs,
roles
ligands
supports
determining
activity,
selectivity,
stability
APMCs
illustrated.
Finally,
some
personal
perspectives
further
development
for
presented.
Nature Communications,
Journal Year:
2021,
Volume and Issue:
12(1)
Published: May 21, 2021
Tuning
metal-support
interaction
has
been
considered
as
an
effective
approach
to
modulate
the
electronic
structure
and
catalytic
activity
of
supported
metal
catalysts.
At
atomic
level,
understanding
structure-activity
relationship
still
remains
obscure
in
heterogeneous
catalysis,
such
conversion
water
(alkaline)
or
hydronium
ions
(acid)
hydrogen
(hydrogen
evolution
reaction,
HER).
Here,
we
reveal
that
fine
control
over
oxidation
states
single-atom
Pt
catalysts
through
significantly
modulates
activities
either
acidic
alkaline
HER.
Combined
with
detailed
spectroscopic
electrochemical
characterizations,
is
established
by
correlating
acidic/alkaline
HER
average
state
Pt-H/Pt-OH
interaction.
This
study
sheds
light
on
atomic-level
mechanistic
HER,
further
provides
guidelines
for
rational
design
high-performance
Journal of the American Chemical Society,
Journal Year:
2021,
Volume and Issue:
143(46), P. 19417 - 19424
Published: Nov. 15, 2021
Single-atom
catalysts
(SACs),
featuring
high
atom
utilization,
have
captured
widespread
interests
in
diverse
applications.
However,
the
single-atom
sites
SACs
are
generally
recognized
as
independent
units
and
interplay
of
adjacent
is
largely
overlooked.
Herein,
by
direct
pyrolysis
MOFs
assembled
with
Fe
Ni-doped
ZnO
nanoparticles,
a
novel
Fe1-Ni1-N-C
catalyst,
neighboring
Ni
pairs
decorated
on
nitrogen-doped
carbon
support,
has
been
precisely
constructed.
Thanks
to
synergism
pairs,
presents
significantly
boosted
performances
for
electrocatalytic
reduction
CO2,
far
surpassing
Fe1-N-C
Ni1-N-C
separate
or
single
atoms.
Additionally,
also
exhibits
superior
performance
excellent
CO
selectivity
durability
Zn-CO2
battery.
Theoretical
simulations
reveal
that,
Fe1-Ni1-N-C,
atoms
can
be
highly
activated
via
non-bonding
interaction,
facilitating
formation
COOH*
intermediate
thereby
accelerating
overall
CO2
reduction.
This
work
supplies
general
strategy
construct
containing
multiple
metal
species
reveals
vital
importance
communitive
effect
between
toward
improved
catalysis.
Joule,
Journal Year:
2022,
Volume and Issue:
6(1), P. 92 - 133
Published: Jan. 1, 2022
Artificial
photocatalytic
energy
conversion
represents
a
highly
intriguing
strategy
for
solving
the
crisis
and
environmental
problems
by
directly
harvesting
solar
energy.
The
development
of
efficient
photocatalysts
is
central
task
pushing
real-world
application
reactions.
Due
to
maximum
atomic
utilization
efficiency
distinct
advantages
outstanding
catalytic
activity,
single-atom
catalysts
(SACs)
have
emerged
as
promising
candidates
photocatalysts.
In
current
review,
recent
progresses
challenges
on
SACs
systems
are
presented.
Fundamental
principles
focusing
charge
separation/transfer
molecular
adsorption/activation
photocatalysis
systemically
explored.
We
outline
how
isolated
reactive
sites
facilitate
photogenerated
electron–hole
transfer
promote
construction
photoactivation
cycles.
widespread
adoption
in
diverse
reactions
also
comprehensively
introduced.
By
presenting
these
advances
addressing
some
future
with
potential
solutions
related
integral
over
SACs,
we
expect
shed
light
forthcoming
research
conversion.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(40), P. 18155 - 18174
Published: Sept. 29, 2022
Single-atom-site
catalysts
(SASCs)
featuring
maximized
atom
utilization
and
isolated
active
sites
have
progressed
tremendously
in
recent
years
as
a
highly
prosperous
branch
of
catalysis
research.
Varieties
SASCs
been
developed
that
show
excellent
performance
many
catalytic
applications.
The
major
goal
SASC
research
is
to
establish
feasible
synthetic
strategies
for
the
preparation
high-performance
catalysts,
achieve
an
in-depth
understanding
active-site
structures
mechanisms,
develop
practical
with
industrial
value.
This
Perspective
describes
up-to-date
development
related
such
dual-atom-site
(DASCs)
nano-single-atom-site
(NSASCs),
analyzes
current
challenges
encountered
by
these
applications,
proposes
their
possible
future
path.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
33(50)
Published: April 2, 2021
Abstract
Lithium–sulfur
(Li‐S)
batteries
have
a
high
specific
energy
capacity
and
density
of
1675
mAh
g
−1
2670
Wh
kg
,
respectively,
rendering
them
among
the
most
promising
successors
for
lithium‐ion
batteries.
However,
there
are
myriads
obstacles
in
practical
application
commercialization
Li‐S
batteries,
including
low
conductivity
sulfur
its
discharge
products
(Li
2
S/Li
S
),
volume
expansion
electrode,
polysulfide
shuttle
effect.
Hence,
immense
attention
has
been
devoted
to
rectifying
these
issues,
which
metal‐based
compounds
(i.e.,
transition
metal,
metal
phosphides,
sulfides,
oxides,
carbides,
nitrides,
phosphosulfides,
MXenes,
hydroxides,
metal‐organic
frameworks)
as
hosts
is
profiled
fascinating
strategy
hinder
effect
stemming
from
polar–polar
interactions
between
polysulfides.
This
review
encompasses
fundamental
electrochemical
principles
insights
into
polysulfides,
with
emphasis
on
intimate
structure–activity
relationship
corroborated
theoretical
calculations.
Additionally,
integration
conductive
carbon‐based
materials
ameliorate
existing
adsorptive
abilities
compound
systematically
discussed.
Lastly,
challenges
prospects
toward
smart
design
catalysts
future
development
presented.
Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(9), P. 6257 - 6358
Published: March 21, 2023
The
oxygen
evolution
reaction
(OER)
and
reduction
(ORR)
are
core
steps
of
various
energy
conversion
storage
systems.
However,
their
sluggish
kinetics,
i.e.,
the
demanding
multielectron
transfer
processes,
still
render
OER/ORR
catalysts
less
efficient
for
practical
applications.
Moreover,
complexity
catalyst–electrolyte
interface
makes
a
comprehensive
understanding
intrinsic
mechanisms
challenging.
Fortunately,
recent
advances
in
situ/operando
characterization
techniques
have
facilitated
kinetic
monitoring
under
conditions.
Here
we
provide
selected
highlights
mechanistic
studies
with
main
emphasis
placed
on
heterogeneous
systems
(primarily
discussing
first-row
transition
metals
which
operate
basic
conditions),
followed
by
brief
outlook
molecular
catalysts.
Key
sections
this
review
focused
determination
true
active
species,
identification
sites,
reactive
intermediates.
For
in-depth
insights
into
above
factors,
short
overview
metrics
accurate
characterizations
is
provided.
A
combination
obtained
time-resolved
information
reliable
activity
data
will
then
guide
rational
design
new
Strategies
such
as
optimizing
restructuring
process
well
overcoming
adsorption-energy
scaling
relations
be
discussed.
Finally,
pending
current
challenges
prospects
toward
development
homogeneous
presented.
